Dynamics of coherence, localization and excitation transfer in disordered nanorings
arXiv:1707.01390 · doi:10.1039/C7CP03171H
Abstract
Self-assembled supramolecular aggregates are excellent candidates for the design of efficient excitation transport devices. Both artificially prepared and natural photosynthetic aggregates in plants and bacteria present an important degree of disorder that is supposed to hinder excitation transport. Besides, molecular excitations couple to nuclear motion affecting excitation transport in a variety of ways. We present an exhaustive study of exciton dynamics in disordered nanorings with long-range interactions under the influence of a phonon bath and take the LH2 system of purple bacteria as a model. Nuclear motion is explicitly taken into account by employing the Davydov ansatz description of the polaron and quantum dynamics are obtained using a time-dependent variational method. We reveal an optimal exciton-phonon coupling that suppresses disorder-induced localization and facilitate excitation de-trapping. This excitation transfer enhancement, mediated by environmental phonons, is attributed to energy relaxation toward extended, low-energy excitons provided by the precise LH2 geometry with anti-parallel dipoles and long-range interactions. An analysis of localization and spectral statistics is followed by dynamical measures of coherence and localization, transfer efficiency and superradiance. Linear absorption, 2D photon-echo spectra and diffusion measures of the exciton are examined to monitor the diffusive behavior as a function of the strengths of disorder and exciton-phonon coupling.
arXiv comment18 pages, 13 figures
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- Simulation of ab initio optical absorption spectrum of β-carotene with fully resolved S_{0} and S_{2} vibrational normal modes
- Diffusion of excitation and power-law localization in long-range-coupled strongly disordered systems
- From Stochastic Hamiltonian to Quantum Simulation: Exploring Memory Effects in Exciton Dynamics